Freeze the dynamicity: charge transfer complexation assisted control over the reaction pathway

Singha, Nilotpal; Pramanik, Bapan; Das, Saurav; Das, Debapratim

doi:10.1039/c9sc03417j

Cited by 18 publications

(9 citation statements)

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“…The understanding of the supramolecular processes involved in the peptide assemblies also opened up the possibility of creating new generation of smart soft-materials with wide range of applications ( Figure 1 ) ( Ahmed et al, 2017 ; Lampel et al, 2018 ; Tian et al, 2018 ; Singha et al, 2019a ; Singha et al, 2019b ; Dasgupta and Das, 2019 ; Tarvirdipour et al, 2020 ). Amongst different types of applications of peptide hydrogels, their use in biomedical or therapeutic purposes holds the major share( Chen and Zou, 2019 ).…”

Section: Introductionmentioning

confidence: 99%

Rational Design of Peptide-based Smart Hydrogels for Therapeutic Applications

Das

2021

Front. Chem.

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Peptide-based hydrogels have captivated remarkable attention in recent times and serve as an excellent platform for biomedical applications owing to the impressive amalgamation of unique properties such as biocompatibility, biodegradability, easily tunable hydrophilicity/hydrophobicity, modular incorporation of stimuli sensitivity and other functionalities, adjustable mechanical stiffness/rigidity and close mimicry to biological molecules. Putting all these on the same plate offers smart soft materials that can be used for tissue engineering, drug delivery, 3D bioprinting, wound healing to name a few. A plethora of work has been accomplished and a significant progress has been realized using these peptide-based platforms. However, designing hydrogelators with the desired functionalities and their self-assembled nanostructures is still highly serendipitous in nature and thus a roadmap providing guidelines toward designing and preparing these soft-materials and applying them for a desired goal is a pressing need of the hour. This review aims to provide a concise outline for that purpose and the design principles of peptide-based hydrogels along with their potential for biomedical applications are discussed with the help of selected recent reports.

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Section: Introductionmentioning

confidence: 99%

Rational Design of Peptide-based Smart Hydrogels for Therapeutic Applications

Das

2021

Front. Chem.

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“…It was reported that copper can act as a catalyst in oxidation reaction in polymer, which can accelerate the generation of perhydrates as following procedure 3,32 . As discussed above, 1024 shown the best anti-oxidation effect in the presence of copper in comparison with 3110 and 1010 for LDPE, which was attributed to the metal-ligand interactions between hydrazide group and copper ions to prevent the further oxidation of materials 10,33 . Therefore, computation simulation was used to confirm the existence of complex.…”

Section: Resultsmentioning

confidence: 88%

Investigation of hindered phenol antioxidant effects on the aging performance of cross-linked LDPE in the presence of copper

Li¹,

Zhou

et al. 2020

Sci Rep

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In this study, LDPE materials with different kinds of antioxidants were prepared by melt-blending method. To reveal the aging mechanism and the anti-oxidation efficiency of LDPE in the presence of copper, series of characterizations including tensile testing, Fourier transform infrared spectra (FTIR), differential scanning calorimetry (DSC), scanning electronic microscopy (SEM) and computation simulation were performed. The experimental results indicated that the aging process significantly decreased the tensile strength and elongation of those aged samples except 1024, which retarded the aging degradation of LDPE at the same condition. These results were further confirmed by the FTIR analysis with the carbonyl index values. Additionally, the melting peaks of DSC plots became broader and shifted to the lower temperatures during the aging process for S-0, S-3114 and S-1010, whereas no obvious changes were observed for S-1024. Importantly, according to the results obtained from computation simulation, a strong metal-ligand interaction between hydrazide group and copper ions was formed to prevent the further oxidation, which accounted for the excellent anti-oxidation behavior of 1024 for LDPE in the presence of copper. Comparing with general organic polyolefin, polyethylene (PE) has excellent temperature resistance, electrical insulation, dielectric properties and weather resistance due to its long chains with regular CH 2 units. Over the past decades, PE materials have been widely used in various areas, such as medical and health, aerospace, wire and cable, automotive industry, architecture and so on 1-4. Unfortunately, it was found that the chemical structure and composition of PE can be significantly destroyed as a result of the comprehensive factors including crosslinking byproducts, metal impurities, ionic impurities, electrical and mechanical effects, moisture, and chemical substances, which result in the failure of the insulation performance 5,6. For example, it has been reported that thermal aging can lead to the deterioration of electrical and mechanical properties of PE insulation 3,7,8. As discussed above, the introduced metal impurities by the process of manufacturing or the operating can lead to the degradation or even failure of PE insulation 3. The metallic impurities consisting of copper powders, originated from the conductor or the ground water, could form heterocharges, which play a role of enhancing the electric stress and promoting the initiation of water tress, and thus decreasing the strength of the PE insulation. As claimed by Gillen 9 , copper powders could diffuse in ethylene propylene rubber(EPR) insulation matrix during the extrusion process, which can account for the degradation of insulation materials during the thermal aging. The introduction of antioxidant into hydrotalcite can shorten the oxidation induction time, which was indicative of the protective action towards oxidation of polymer, whereas, the impurity of hydrotalcite and metal ions can increase the rate of polypropylene photo...

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“…Recently, we have shown the effect of molecular arrangement of two thiol molecules (in the aggregated state) on the disulfide formation possibility. 15 It was found that the thiol groups need to be in a very close proximity (∼4 Å) in order to form the disulfide bonds. Following our previous report, energy minimized structures for two molecules of the same peptides are obtained using DFT calculation.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Short peptide based self-assembled systems are receiving significant current interest as biomaterials, mainly because of their biocompatibility and degradability. − These smart soft materials have found applications in various fields, including drug delivery, , matrix for cell proliferation, , protective storage of proteins, sensors, , nanofabrication, − organic methodology, , and organic electronics, to name a few. One of the most common outcomes of the self-assembly of these short peptides is the formation of hydrogels. , According to need, with proper permutation and combination of the constituent amino acids, the properties of these hydrogels can be altered.…”

Section: Introductionmentioning

confidence: 99%

Smart Thixotropic Hydrogels by Disulfide-Linked Short Peptides for Effective Three-Dimensional Cell Proliferation

et al. 2020

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Supramolecular assembly of short peptides is a crucial process and has shown numerous potential applications as biomaterials. In the present work, the hydrogelation process of short peptides containing C-terminal “Lys–Cys” (KC) residues have been studied in detail. The N-terminal capping is found to be essential for effective gelation. Out of 12 peptides we studied, two of them could form hydrogels efficiently: Ac-VVKC-NH2 and Ac-FFKC-NH2. In both cases, the monomer-to-dimer formation through disulfide linkages by Cys residues controls the aggregation process. Interestingly, the presence of H2O2 facilitated the dimerization and thereby reduced the gelation time but could not impart much effect on the mechanical properties of the gels. Detailed rheological study revealed that both hydrogels are thixotropic in nature. Moreover, they are responsive to glutathione (GSH) due to the presence of disulfide linkages. However, the hydrogel of Ac-FFKC-NH2 is found to be stronger and more effective for biological applications. The thixotropic nature as well as a model drug release study in response to varying GSH concentration indicates the possible use of the hydrogel as an injectable local drug delivery vehicle. The hydrogel of Ac-FFKC-NH2 is noncytotoxic in nature. Three-dimensional cell proliferation has been found to be more effective than 2D, as it mimics the in vivo situation more closely if not exactly. In the present study, we have shown that both differentiated RAW macrophages and undifferentiated THP-1 monocytes could proliferate significantly within the 3D matrix of the hydrogel, without depicting any apparent cytotoxicity. Thus, the hydrogel of Ac-FFKC-NH2 has potential for application in localized drug administration and as a supporting biomaterial to study basic phenomena involving cell behavior.

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Freeze the dynamicity: charge transfer complexation assisted control over the reaction pathway

Abstract: Aqueous CT complexes of donor and acceptor molecules with reactive thiol groups were frozen and lyophilized to get alternate D–A assemblies in the solid state. Oxidation of the thiols resulted in asymmetric disulfides exclusively.

Cited by 18 publications

References 35 publications

Rational Design of Peptide-based Smart Hydrogels for Therapeutic Applications

Rational Design of Peptide-based Smart Hydrogels for Therapeutic Applications

Investigation of hindered phenol antioxidant effects on the aging performance of cross-linked LDPE in the presence of copper

Smart Thixotropic Hydrogels by Disulfide-Linked Short Peptides for Effective Three-Dimensional Cell Proliferation

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